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Porous single layer molybdenum disulfide (MoS$_2$) is a promising material for applications such as DNA sequencing and water desalination. In this work, we introduce irradiation with highly charged ions (HCIs) as a new technique to fabricate well-defined pores in MoS$_2$. Surprisingly, we find a linear increase of the pore creation efficiency over a broad range of potential energies. Comparison to atomistic simulations reveals the critical role of energy deposition from the ion to the material through electronic excitation in the defect creation process, and suggests an enrichment in molybdenum in the vicinity of the pore edges at least for ions with low potential energies. Analysis of the irradiated samples with atomic resolution scanning transmission electron microscopy reveals a clear dependence of the pore size on the potential energy of the projectiles, establishing irradiation with highly charged ions as an effective method to create pores with narrow size distributions and radii between ca. 0.3 and 3 nm., Comment: 22 pages, 4 figures

We report a simple technique for the selective etching of bilayer and monolayer MoS$_2$. In this work, chosen regions of MoS$_2$ were activated for oxygen adsorption and reaction by the application of low doses of He$^+$ at 30 keV in a gas ion microscope. Raman spectroscopy, optical microscopy and scanning electron microscopy were used to characterize both the etched features and the remaining material. It has been found that by using a pre-treatment to introduce defects, MoS$_2$ can be etched very efficiently and with high region specificity by heating in air., Comment: 8 pages, 6 figures

We investigate the effects of lattice disorders on the low frequency Raman spectra of bilayer MoS2. The bilayer MoS2 was subjected to defect engineering by irradiation with a 30 keV He+ ion beam and the induced morphology change was characterized by transmission electron microscopy. With increasing ion dose the shear mode is observed to redshift and it is also suppressed sharply compared to other Raman peaks. We use the linear chain model to describe the changes to the Raman spectra. Our observations suggest that crystallite size and orientation are the dominant factors behind the changes to the Raman spectra., Comment: 5 pages, 4 figures in main paper + supplemental

Field-effect transistors (FETs) with non-covalently functionalised molybdenum disulfide (MoS2) channels grown by chemical vapour deposition (CVD) on SiO2 are reported. The dangling-bond-free surface of MoS2 was functionalised with a perylene bisimide derivative to allow for the deposition of Al2O3 dielectric. This allowed the fabrication of top-gated, fully-encapsulated MoS2 FETs. Furthermore, by the definition of vertical contacts on MoS2, devices, in which the channel area was never exposed to polymers, were fabricated. The MoS2 FETs showed high mobilities for transistors fabricated on SiO2 with Al2O3 as top-gate dielectric. Thus, gate-stack engineering using innovative chemistry is a promising approach for the fabrication of reliable electronic devices based on 2D materials.

Precise and scalable defect engineering of 2D nanomaterials is acutely sought-after in contemporary materials science. Here we present defect engineering in monolayer graphene and molybdenum disulfide (MoS$_2$) by irradiation with noble gas ions at 30 keV. Two ion species of different masses were used in a gas field ion source microscope: helium (He$^+$) and neon (Ne$^+$). A detailed study of the introduced defect sizes and resulting inter-defect distance with escalating ion dose was performed using Raman spectroscopy. Expanding on existing models, we found that the average defect size is considerably smaller for supported than freestanding graphene and that the rate of defect production is larger. We conclude that secondary atoms from the substrate play a significant role in defect production, creating smaller defects relative to those created by the primary ion beam. Furthermore, a similar model was also applied to supported MoS$_2$, another promising member of the 2D material family. Defect yields for both ions were obtained for MoS$_2$, demonstrating their different interaction with the material and facilitating comparison with other irradiation conditions in the literature., Comment: 11 pages, 6 figures

Molybdenum disulfide (MoS2) is a particularly interesting member of the family of two-dimensional (2D) materials due to its semiconducting and tunable electronic properties. Currently, the most reliable method for obtaining high-quality industrial scale amounts of 2D materials is chemical vapor deposition (CVD), which results in polycrystalline samples. As grain boundaries (GBs) are intrinsic defect lines within CVD-grown 2D materials, their atomic structure is of paramount importance. Here, through atomic-scale analysis of micrometer-long GBs, we show that covalently bound boundaries in 2D MoS2 tend to be decorated by nanopores. Such boundaries occur when differently oriented MoS2 grains merge during growth, whereas the overlap of grains leads to boundaries with bilayer areas. Our results suggest that the nanopore formation is related to stress release in areas with a high concentration of dislocation cores at the grain boundaries, and that the interlayer interaction leads to intrinsic rippling at the overlap regions. This provides insights for the controlled fabrication of large-scale MoS 2 samples with desired structural properties for applications., Comment: 26 pages, including supplementary material

Platinum diselenide (PtSe2) is a newly discovered 2D material which is of great interest for applications in electronics and catalysis. PtSe2 films were synthesized by thermally-assisted selenization of predeposited platinum films and scanning transmission electron microscopy revealed the crystal structure of these films to be 1T. Raman scattering of these films was studied as a function of film thickness, laser wavelength and laser polarization. Eg and A1g Raman active modes were identified using polarization measurements in the Raman setup. These modes were found to display a clear position and intensity dependence with film thickness, for multiple excitation wavelengths, and their peak positions agree with simulated phonon dispersion curves for PtSe2. These results highlight the practicality of using Raman spectroscopy as a prime characterization technique for newly-synthesized 2D materials.

Transition metal dichalcogenides (TMDs) have recently attracted attention due to their interesting electronic and optical properties. Fabrication of these materials in a reliable and facile method is important for future applications, as are methods to characterize material quality. Here we present the chemical vapor deposition of MoSe2 monolayer and few layer crystals. These results show the practicality of using chemical vapor deposition to reliably fabricate these materials. Low frequency Raman spectra and mapping of shear and layer breathing modes of MoSe2 are presented for the first time. We correlate the behavior of these modes with layer number in the materials. The usefulness of low frequency Raman mapping to probe the symmetry, quality, and monolayer presence in CVD grown 2D materials is emphasized.

The optical nonlinearity of WS2, MoS2 monolayer and few-layer films was investigated using the Z-scan technique with femtosecond pulses from the visible to the near infrared. The dependence of nonlinear absorption of the WS2 and MoS2 films on layer number and excitation wavelength was studied systematically. WS2 with 1~3 layers exhibits a giant two-photon absorption (TPA) coefficient. Saturation of TPA for WS2 with 1~3 layers and MoS2 with 25~27 layers was observed. The giant nonlinearity of WS2 and MoS2 is attributed to two dimensional confinement, a giant exciton effect and the band edge resonance of TPA.